SURFACE & COATINGS TECHNOLOGY
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2024
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IF 5.3
Guangyin Liu,Yuhui Zhang,Chaofan Ma,Qin Tang,Hanbing Li,Shiqi Chen,Jun Shen
The gallium (Ga) base liquid metal (LM) with high thermal conductivity and deformability is applied widely in thermal management in electrical systems. However, Ga readily reacts with Cu to form intermetallic compounds (IMCs), which can cause failure in electronic devices. Herein, the thermal interface material (TIM) with Ga and diamond is prepared to analyze the reaction behavior of TIM and Cu/Ni-plated Cu under an aging test at 125 °C. The results show that Ga reacts with Cu substrate and forms CuGa 2 bulk. Moreover, Ni coating can inhibit the corrosion of Ga and Cu. However, the as-volcano IMC structures were generated, also. The thermal resistance increased from 2.24 mm 2 ·K·W −1 to 14.47 mm 2 ·K·W −1 from initial time to 200 h. The interfacial corrosion behavior between TIM and Cu substrate is studied by first-principles molecular dynamics simulation. The diffusion coefficient in the z direction of Cu is 0.04 × 10 −5 cm 2 /s. In a word, the work could provide the guidelines for the further design of high-performance corrosion resistance in the region where Ga was used for thermal management on electronic products.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Jianshe Zhang,Chunling Zheng,Yingjie Wang,Tingting Zhai,Yanghuan Zhang,Dianchen Feng
This research paper explores the influence of varying the quantity of La–Ni@3DG catalyst on the hydrogen storage capabilities of MgH 2 . La–Ni@3DG catalyst was prepared using lanthanum chloride heptahydrate and nickel chloride hexahydrate as raw materials combined with three-dimensional graphene, then mixed with MgH 2 via ball milling to prepare MgH 2 + x wt.% La–Ni@3DG ( x = 0, 3, 5, 7) composite alloy. X-ray diffraction analysis showed that the composite alloy was mainly composed of the MgH 2 phase, with the presence of Mg and (La, Ni) phases detected. With increased La–Ni@3DG addition, the broadening of the MgH 2 diffraction peak significantly improved, indicating the catalyst promoted alloy phase structure uniformity and crystallinity. The composite alloy forms new phases such as LaH 3 , LaNi 3 H 6 , and Mg 2 NiH 4 during hydrogen absorption. These phases cooperate with in-situ formed LaH 3 and Mg 2 Ni to significantly improve the reversible hydrogen absorption and desorption properties of MgH 2 . Adding La–Ni@3DG catalyst has a significant positive effect on the hydrogen absorption and desorption of MgH 2 , leading to a considerable improvement. At 553 K, the composite alloy reaches hydrogen absorption equilibrium faster than pure MgH 2 , and the temperature for hydrogen absorption is significantly reduced to 373 K. The dehydrogenation performance is also improved, with 5 wt.% La–Ni@3DG is showing the best dehydrogenation performance at 553 K. The initial dehydrogenation temperature commences at approximately 505 K, while the dehydrogenation activation energy attains its minimum value: a remarkably low 109.91 kJ/mol H 2 . Additionally, the addition of catalyst reduces the pressure of the hydrogen absorption and desorption platform, effectively reducing the hysteresis effect during hydrogen absorption and desorption when the catalyst content is 5 wt.%, the enthalpy change and entropy change of the composite alloy reach a minimum, −70.45 kJ/mol H 2 and 74.38 kJ/mol H 2 (hydrogen absorption), −101.93 J/K/mol H 2 and 103.68 J/K/mol H 2 (hydrogen desorption), respectively.
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Journal of Environmental Sciences
·
2025
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IF 6.3
Yansen Qu,Xin Li,Yingjie Xia,Haosheng Lan,Le Ding,Jing Zhong,Xinghua Chang
Accelerated industrialization combined with over-applied nitrogen fertilizers results in serious nitrate pollution in surface and ground water, disrupting the balance of the global nitrogen cycle. Electrochemical nitrate reduction (eNO 3 RR) emerges as an attractive strategy to simultaneously enable nitrate removal and decentralized ammonia fabrication, restoring the globally perturbed nitrogen cycle. However, complex deoxygenation-hydrogenation processes and sluggish proton-electron transfer kinetics significantly hinder practical application of eNO 3 RR. In this study, we developed carbon-coated Cu-Ni bimetallic catalysts derived from metal-organic frameworks (MOFs) to facilitate eNO 3 RR. The unique structural features of catalyst promote enhanced synergy between Cu and Ni, effectively addressing critical challenges in nitrate reduction. Comprehensive structural and electrochemical analysis demonstrate that electrochemical nitrate-to-nitrite conversion mainly takes place on active Cu sites, the introduction of Ni could efficiently accelerate the generation of aquatic active hydrogen, promoting the hydrogenation of oxynitrides during eNO 3 RR. In addition, Ni introduction could push up the d-band center of the catalyst, thus enhancing the adsorption and activation of nitrate and the corresponding intermediates. Detailed reaction pathways for nitrate-to-ammonia conversion are illuminated by rotating disk electrode (RDE), in-situ Fourier-transform infrared spectroscopy, in-situ Raman spectrum and electrochemical impedance spectroscopy (EIS). Benefiting from the synergistic effect of Cu and Ni, optimum catalyst exhibited excellent nitrate reduction performance. This work provides a new idea for elucidating the underlying eNO 3 RR reaction mechanisms and contributes a promising strategy for designing efficient bimetallic electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Lin Ai,Yanping Chen,Fang Lu,Jiaxu Liu,Xiao-Feng Wu,Shengjun Huang
The fundamental challenge in the gas-phase selective hydrogenation of α,β-unsaturated aldehydes to α,β-unsaturated alcohols lies in the construction of microscopic environment for the preferential hydrogenation of C = O bond along with the preservation of C = C bond under the reductive atmosphere. Herein, we proposed a structure-matching strategy for the catalyst design, in which In component in metallic form and oxide form are interplayed with metallic Ni and Al 2 O 3 support, respectively. The fabrication of In-Ni intermetallic compound stokes up the desirable electropositive-electronegative environment (In δ+ -Ni δ- ) for the adsorption of polar carbonyl group. The In species in the In-oxo form are engaged in the network of Al 2 O 3 support in the formation of In-O-Al-O entities, which stabilizes the heterolytically dissociated H species to match the preferential saturation of polar C = O bond. Therefore, the resulting In-Ni-Al 2 O 3 catalyst achieves a selectivity of 77.2 % to methallyl alcohol with a conversion of 53.8 % in the gas-phase hydrogenation process, which present a striking contrast to the outcomes upon the counterpart Ni-Al 2 O 3 (non-selectivity to methallyl alcohol). Such structure-matching strategy enriches the fundamental understandings and basis for the rational design of catalysts for the selective hydrogenation of unsaturated aldehydes.
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JOURNAL OF THE ENERGY INSTITUTE
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2024
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IF 5.6
Jiawen Chi,Xueqian Wu,Jiangyan Tao,Xin Min,Zhen Li,Songjian Zhao
Climate warming caused by the yearly rise of CO 2 emissions has posed a great challenge to the survival and development of human beings. In this study, the active component Ni was combined with mesoporous silica (SiO 2 ) to construct a highly dispersed Ni composite silicon-based catalyst (Ni x /Si), which was introduced into the dielectric barrier discharge (DBD) system for the conversion of CO 2 . The XRD and FTIR analyses confirmed that Ni was successfully introduced into the SiO 2 carrier and the SEM results showed that the Ni elements were uniformly distributed. BET and TGA results revealed large specific surface area, stable mesoporous structure, and high thermal stability of the prepared Nix/Si. Further investigation of DBD-coupled Ni x /Si performance for CO 2 conversion showed significant variations based on different Ni loadings, with optimal CO 2 conversion rate, CO yield, and energy efficiency achieved at 3% Ni loading, which increased by 121.8%, 101.5%, and 102.4% respectively compared to the SiO 2 support. During the process of reducing CO 2 , the combination of Ni x /Si and DBD exhibited synergistic effects, with Ni 0 playing a crucial role in the CO 2 reduction. The introduction of Ni x /Si enhances charge transfer in the discharge region, improves CO 2 adsorption, and reduces the dissociation energy of CO 2 bonds. The DBD-coupled Ni x /Si developed by this study offers several advantages including low energy consumption, simple operation, and high efficiency, making it a promising solution for CO 2 treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yongzhi Xiong,Shengchun Hu,Jianchun Jiang,Yajun Liu,Wei Zhao,Xialin Ji,Changzhou Chen,Mengmeng Fan,Kui Wang
Herein, a novel ball milling-pyrolysis strategy was proposed for preparing a highly dispersed Ni 3 Fe nanoalloy catalyst (Ni 3 Fe@NC) used for 5-hydroxymethylfurfural (HMF) electro-oxidation reaction. The Ni 3 Fe@NC delivered a high current density of 100 mA cm −2 at a low potential of 1.467 V vs RHE, with a HMF conversion rate of over 99.6 %, 2,5-furan dicarboxylic acid (FDCA) selectivity of 97.1 % and a Faraday efficiency of 96.7 %. Theoretical calculations, in-situ EIS, quasi-in-situ XRD and XPS demonstrated that Fe-doping optimizes the electronic structure of Ni 3 Fe@NC and regulates its d -band center, which not only promoted the reconstruction of Ni 3 Fe@NC to form high-oxidation-activity Ni 2+δ and Ni 3+δ species but also reduced the reaction barrier of the key rate-determining step (*5-Hydroxymethyl-2-furancarboxylic acid (HMFCA)→*5-formyl-2-furancarboxylic acid (FFCA)) during HMFOR. Based on this interesting work, we provided a facile macroscopic preparation strategy on highly dispersed nanoalloy catalyst for efficient electro-oxidation of HMF.
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ADVANCED POWDER TECHNOLOGY
·
2024
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IF 4.2
Zigui Luo,Qi Jin,Rui Wang,Zhenjia Yang,Zhaoyang Wu,Guangqiang Li,Xi’an Fan
FeSiAl/(Al 2 O 3 -Ni) soft magnetic composites (SMCs) were prepared by sintering FeSiAl/NiO composite powders, and the formation mechanism of the Al 2 O 3 -Ni composite coating and performance of the FeSiAl SMCs with different NiO coating content were studied. During sintering, high temperature promoted a reaction between Al and NiO at the FeSiAl/NiO interface, resulting in the in-situ formation of a composite coating comprising Al 2 O 3 coating with high integrity and ferromagnetic Ni coating. The interdiffusion of Al and O 2– toward the interface ensured the continuation of the reaction and growth of the composite coating. The composite coating thickened with the increasing NiO coating content, thus showing reduced real part of permeability. Saturation magnetization considerably increased until the NiO coating content exceeded 12.5 wt% owing to residual NiO. Excessive NiO coating content led to the generation of a large amount of Ni, which was not conducive to the integrity of the Al 2 O 3 coating and increased magnetic loss. The FeSiAl SMCs with 5.0 wt% NiO coating content exhibited exceptional performance with high saturation magnetization (135.3 emu/g), good frequency stability of permeability, and low magnetic loss (63.7 W/kg at 0.05 T/20 kHz).
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ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2024
·Vol. 650
·期 16
·e202400047
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IF 1.1
Zhong-Xuan Xu,Xiu-Ju Ying,Fei Fei
Under hydrothermal condition, lactate derivative ( R )-4-(1- carboxyethoxy)-2-methylbenzoic acid (( R )-H 2 cma) as chiral synthon assembled with 4,4′-di(1H-imidazol-1-yl)-1,1′-biphenyl (4,4’-dib) and Ni(II) ions to obtain complex {[Ni 2 (( R )-cma) 2 (4,4’-dib) 2 (H 2 O)] ⋅ 2H 2 O} n ( HU20- R ). In complex HU20- R , carboxyl group from lactate unit of ( R )-cma 2− anion and coordinating H 2 O molecule adopt a μ 2 -coordination mode to obtain dinuclear [Ni 2 (CO 2 ) 2 (H 2 O)] 2+ cluster. ( R )-cma 2− anions and Ni(II) ions build single left-handed ( R )-cma-Ni-chain, while 4,4’-dib ligands are bridged by different Ni(II) centers to form double left-handed 4,4’-dib-Ni-chain. These helical secondary structures are further connected together to result in an 8-connected 3D framework. PXRD tests indicated that complex HU20- R has well hydro-stability. UV-vis absorption experiment confirmed that HU20- R is a semi-conducting material with strong absorption capacity for ultraviolet-visible (UV-vis) light. Additionally, electrochemical experiment revealed that HU20- R has low impedance and high charge transport capacity. Further test results confirm that HU20- R has noticeable photo-catalytic effect in photodegradation of Rhodamine B (RhB) and antiferromagnetic property.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Long Haoyu,Zhang Xidong,Zhang Zhenyi,Zhang Jianjun,Yu Jiaguo,Yu Huogen
The H 2 -evolution kinetics play a pivotal role in governing the photocatalytic hydrogen-evolution process. However, achieving precise regulation of the H-adsorption and H-desorption equilibrium (H ads /H des ) still remains a great challenge. Herein, we propose a fine-tuning d - p hybridization strategy to precisely optimize the H ads /H des kinetics in a Ni-B x modified CdS photocatalyst (Ni-B x /CdS). X-ray absorption fine-structure spectroscopy and theoretical calculations reveal that increasing B-atom amount in the Ni-B x cocatalyst gradually strengthens the d - p orbital interaction between Ni 3 d and B 2 p , resulting in a consecutive d -band broadening and controllable d -band center on Ni active sites. The above consecutive d -band optimization allows for precise modulation of the H ads /H des dynamics in the Ni-B x /CdS, ultimately demonstrating a remarkable H 2 -evolution activity of 13.4 mmol g -1 h -1 (AQE = 56.1 %). The femtosecond transient absorption spectroscopy further confirms the rapid electron-transfer dynamics in the Ni-B x /CdS photocatalyst. This work provides insights into the optimal design of prospective H 2 -evolution catalysts.
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BIOMASS & BIOENERGY
·
2024
·
IF 5.8
Yacong Deng,Yanlin Xu,Zhuoyi Liu,Wenhong Wang,Bin Liu,Hailing Guo,Yanpeng Li,Bin Dong,Yichuan Li,Yuan Pan,Yongming Chai,Chenguang Liu
The efficient utilization of lignin from the papermaking black liquor has attracted interest due to its carbon-neutral value and industrial application. This work illustrates a simple support-phosphate-pretreatment strategy to develop superdispersed Ni species in activated carbon (AC) to enhance the hydrodeoxygenation (HDO) reactions of the lignin model compound guaiacol into biohydrocarbons under alkaline conditions. For the first time, sodium polyphosphate was applied as a pretreatment agent for coconut carbon in the synthesis of carbon-supported Ni catalysts. Superdispersed Ni nanoparticles were achieved on Ni/NaP n OAC with a particle size of 2.5 nm, which was much smaller than that on unmodified Ni/C (13.1 nm). The characterization results and reactions revealed that the P−O that formed served as anchoring sites for the Ni species and strengthened the interaction between the Ni species and support (SMSI), which resulted in significantly improved dispersion of the Ni metal sites and, thus, a nearly 6-fold greater yield of hydrocarbons was obtained on Ni/NaP n OAC (58.1 %) than on Ni/C (10.1 %). In addition, compared with Ni 2 P/NaP n OAC and NiS/NaP n OAC, Ni/NaP n OAC exhibited higher HDO activity, especially higher direct deoxygenation (DDO) activity and higher benzene yield, reducing hydrogen consumption during the HDO reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiaomeng Yang,Fei Geng,Zhanghan Shi,Dan Wu,Armin Rezayan,Jingpeng Zhao,Renfeng Nie,Jianshe Wang,Chunbao Xu,Yongsheng Zhang
Reductive etherification of carbonyl compounds using metal–acid bifunctional catalysts is an important strategy for the synthesis of ethers. Conventional metal–acid bifunctional catalysts suffer from poor synergistic effects due to the spatially separated distribution of hydrogenation sites on metal nanoparticles and acid sites on supports. In this study, bifunctional Ni-I catalysts with intimate metal–acid bifunctional sites were prepared through the surface modification of Ni nanoparticles with organic iodide under H 2 atmosphere. Hydrogenolysis of C-I bonds over Ni nanoparticles promotes the selective deposition of I atoms on the Ni surface. Electronegative I atoms withdraw electrons from Ni nanoparticles, which enables the heterolytic dissociation of H 2 over Ni-I polar sites, leading to the in-situ generation of Ni(H - )-I(H + ) bifunctional sites on the metal surface. The reductive etherification of furfural and ethanol over Ni-I bifunctional catalysts demonstrated high efficiency with an 89.4 % yield to furfuryl ethyl ether (FEE) at mild reaction conditions. Mechanistic studies revealed that both the selective deactivation effect and the in-situ generation of Brønsted acidity contribute to this reaction pathway. While the I atoms selectively deactivate the consecutive Ni sites, suppressing the over-hydrogenation of the furan ring, the in-situ generated Brønsted acid sites catalyze the acetalization. Furthermore, temperature-programmed pyridine FTIR analysis revealed that the Brønsted acidity on the Ni-I catalyst is only evident at high temperatures (e.g., over 100°C) due to the high dissociation energy required for H 2 on non-noble metal surfaces. The developed Ni-I bifunctional catalysts, featuring intimate metal–acid sites and low-cost, holds great promise for the catalytic upgrading of biomass-derived oxygenates into fine chemicals.
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JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Tao Chen,Fei Shan,Lingting Ye,Kui Xie
Due to their excellent high Faraday efficiency, perovskite solid oxide cells (SOECs) have attracted considerable attention. Nevertheless, they still face significant challenges in terms of stability and electrocatalytic activity during CO₂ electrolysis. In this study, Ni particles in La 0.65 Ba 0.35 Mn 1-x Ni x O 3-δ are successfully separated by a unique in-situ exsolved method of metal nanoparticles, which are uniformly anchored to the electrode surface as Ni nanometal particles. This effectively suppresses the generation of carbon deposits on the cathode surface. Under test conditions of 850 °C, 1.6 V and 50 sccm flow rate, the CO yield of the modified cathode material reached 5.9 mL min −1 cm −2 , which is nearly four times higher than that before doping. The synergistic effect of in-situ exsolution of Ni metal nanoparticles with oxygen defects generated by the perovskite, creating more active locations for CO 2 adsorption and electrolysis, is responsible for the significant improvement in electrochemical performance. This work provides new strategies and ideas for the development of efficient and durable SOEC cathode materials.
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